This study investigated breed-specific flavor characteristics in Guanling (GL), Sinan (SN), and Simmental-crossbred (XZ) cattle using UHPLC-MS/MS and GC × GC-TOF MS. Specifically, XZ had 73 and 48 differential metabolites compared to GL and SN, respectively, whereas GL and SN showed 31 discriminated metabolites. Notably, these differences were linked to flavor-related metabolic pathways, particularly beta-alanine, histidine, glutathione, and purine metabolism. Regarding the composition of volatile organic compounds (VOCs), GL displayed a higher ketone content (18.58 %), whereas XZ was enriched in alcohol (56.25 %). Key VOCs with the highest flavor contributions across all breeds were 2,3-Butanedione, (E)-2-nonenal, 2-ethyl-1-hexanol, and (E)-2-octenal. However, dimethyl sulfide contributed significantly to GL and SN flavors but not to XZ. Collectively, the 49 differential VOCs led to aroma profiles of breeds varied in "sweet", "fruity", "nutty", and "waxy" characteristics. This comprehensive analysis of non-volatile metabolites and flavor-related VOCs revealed breed-specific profiles and crossbreeding effects, providing insights for improving meat quality.